CN101752557A - Pr5Co19 type cathode hydrogen storage material and application thereof - Google Patents
Pr5Co19 type cathode hydrogen storage material and application thereof Download PDFInfo
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- CN101752557A CN101752557A CN200810181720A CN200810181720A CN101752557A CN 101752557 A CN101752557 A CN 101752557A CN 200810181720 A CN200810181720 A CN 200810181720A CN 200810181720 A CN200810181720 A CN 200810181720A CN 101752557 A CN101752557 A CN 101752557A
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Abstract
The invention provides a Pr5Co19 type cathode hydrogen storage material, which has atomic ratio components of La0.75-x-yNdxDyyMg0.25Ni3.27Al0.13, wherein x is not less than 0.1 and not more than 0.3, and y is not less than 0.01 and is not more than 0.05. The Pr5Co19 type cathode hydrogen storage material can be used as a negative electrode and used for preparing a nickel-metal hydride battery with high capacity.
Description
Technical field
The present invention relates to Pr
5Co
19The type nickel-hydrogen battery negative electrode hydrogen storage material.Especially, Pr involved in the present invention
5Co
19The type cathode hydrogen storage material is than present existing AB
5The commercial capacity with hydrogen storage material of type is higher, therefore is specially adapted to the preparation of high-capacity nickel-hydrogen battery.
Technical background
Metal hydride-nickel cell is since last century, put goods on the market the nineties, because it is long that it has capacity height, life-span, characteristics such as memory-less effect, non-environmental-pollution, extensively receive an acclaim, occupation rate of market is more and more higher, cell types is also developed to other polytypes by AA, AAA common batteries, and product is widely used in electric tool, household electrical appliance, computer, space flight, communication and vehicle using motor etc., develops very rapid.Along with the increase of metal hydride-nickel cell application, also more and more higher to the requirement of battery performance.The development of particularly wireless in recent years chargeable electric tool and electric automobile is had higher requirement to the capacity of metal hydride-nickel cell.
The capacity of battery mainly is to be determined by the both positive and negative polarity capacity of battery, and the capacity of raising battery plus-negative plate is the main approach that improves battery capacity, and the electrochemistry capacitance that therefore improves the battery cathode hydrogen storage material just becomes particularly important.AB
5The type hydrogen storage material through years of researches, has been developed a series of AB at present since the commercialization of phase at the end of the eighties in last century
5Type hydrogen storage alloy, properties of product also are greatly improved, the electrochemistry capacitance of hydrogen storage material is brought up to greater than 330mAh/g by initial 260mAh/g, the capacity of metal hydride-nickel cell (in AA) is also brought up to 2700mAh from about initial 1000mAh, one of reason that though the raising of positive electrode capacity and the change of battery structure also are battery capacities to improve, but the raising of cathode hydrogen storage material capacity also plays an important role, therefore to further improve the capacity of battery, just must further improve the capacity of negative or positive electrode, because the capacity of the employed anodal hickelous nydroxide of metal hydride-nickel cell improves limited at present, therefore people just have been placed on the research emphasis that improves the metal hydride-nickel cell capacity above the research of cathode hydrogen storage material, for LaNi
5The type hydrogen storage material, experiment shows that it is 6 hydrogen atoms that the maximum of common every unit cell is inhaled number of hydrogen atoms, thus according to Theoretical Calculation as can be known its theoretical electrochemistry capacity be 372mAh/g, for the hydrogen storage material of commerce usefulness, for the performance of improving product is used needs, LaNi to satisfy
5In the mixed rare earth Mm of Rare Earth Lanthanum (La) substitute, nickel (Ni) is by cobalt (Co), manganese (Mn) and aluminium (Al) part are alternative, typical composition is MmNi
3.55Co
0.75Mn
0.4Al
0.3, this electrochemistry capacitance that makes material inevitably that substitutes descends, and its theoretical capacity is considered to 348mAh/g, thereby makes people recognize further raising AB
5Therefore the electrochemistry capacitance potentiality of type hydrogen storage material are little, the exploitation of high power capacity storage hydrogen material concentrated on the product of other types, and people begin one's study one after another and have the more hydrogen storage material of high power capacity, as with ZrMn
2AB for representative
2Type Laves phase alloy is the AB type of representative and with Mg with TiFe
2Ni is the A of representative
2B magnesium base alloy, but up to now, these materials be owing to exist the problem (still unresolved as problems such as activity function and life-spans) of various aspects, thereby still be in conceptual phase, still untappedly goes out practical product, and add the AB of Mg
3.5Type La
1-xMg
xNi
3.5Hydrogen storage material is because theoretical capacity surpasses 400mAh/g, and good activation characteristic is arranged, and becomes the Recent study hot of research and development.
Therefore, for satisfying the needs of high-capacity nickel-hydrogen battery product, the applicant is with La
1-xMg
xNi
3.5Be research object, by adding different element kinds therein, thereby proposed a kind of with Pr
5Co
19Type crystal structure is the main cathode hydrogen storage material that uses for nickel-hydrogen battery with high charge-discharge capacity.
Summary of the invention
The objective of the invention is to obtain the much higher cathode hydrogen storage material of a kind of ratio present commercially available prod charge discharge capacity, to satisfy the demand of high-capacity nickel-hydrogen battery product by the composition improvement.
Specifically, the invention provides a kind of Pr that is applicable to Ni-MH battery
5Co
19The type cathode hydrogen storage material, it has the high electrochemical charge/discharge capacity, this Pr
5Co
19The atomic ratio composition of type cathode hydrogen storage material consists of La
0.75-x-yNd
xDy
yMg
0.25Ni
3.27Al
0.13, wherein 0.1≤x≤0.3,0.01≤y≤0.05.
Pr
5Co
19Type cathode hydrogen storage material and AB
5Hydrogen storage material equally is that elements A by easy generation stable hydride is (as La, Nd, Mg etc.) with other element B (as Ni, Al, Mn, Co etc.) intermetallic compound of Zu Chenging, its charge discharge capacity mainly comes to inhale to be put in the hydrogen process, and the electron transfer in the oxidation-reduction process takes place on hydrogen-bearing alloy electrode the hydrogen ion in the electrolyte, and the charge discharge reaction ordinary representation of ni-MH battery is as follows:
The charging reaction:
At negative pole, when applying an electrode potential to negative electrode, the water in the electrolyte is broken down into hydrogen ion and hydroxide ion, and hydrogen ion becomes hydrogen atom at cathode hydrogen storage material surface electron gain, is inhaled in the alloy, and hydroxide ion is left in the electrolyte:
Alloy+H
2O+e
-→Alloy[H]+OH
- (1)
Alloy represents hydrogen bearing alloy in the formula.
At positive pole, two valency nickel in the hickelous nydroxide lose an electronics and are oxidized to nickelic and combine with hydroxide ion in the electrolyte and become nickel hydroxide:
Ni(OH)
2+OH
-→NiOOH+H
2O+e
- (2)
Exoelectrical reaction:
At negative pole, be absorbed in that hydrogen in the hydrogen bearing alloy is released and be combined into water with hydroxide ion in the electrolyte, contribute an electronics simultaneously and form electric current.
Alloy[H]+OH
-→Alloy+H
2O+e
- (3)
At positive pole, nickel hydroxide obtains an electronics and is reduced into the lower valency hickelous nydroxide and discharges hydroxide ion and enter in the electrolyte.
NiOOH+H
2O+e
-→Ni(OH)
2+OH
- (4)
Pr of the present invention
5Co
19The type hydrogen storage material can be used for preparing the negative pole of metal hydride-nickel cell.Adopt Pr of the present invention
5Co
19The type cathode hydrogen storage material has very high electrochemical discharge capacity as the metal hydride-nickel cell of negative pole.
With the AB that sells in the market
5The type hydrogen storage material is (as the traditional cathode hydrogen storage material MmNi for preparing with identical smelting technology
3.55Co
0.75Mn
0.4Al
0.3) compare Pr of the present invention
5Co
19Type cathode hydrogen storage material La
0.75-x-yNd
xDy
yMg
0.25Ni
3.27Al
0.13The charge/discharge capacity of (0.1≤x≤0.3,0.01≤y≤0.05) significantly improves.Correspondingly, adopt Pr of the present invention
5Co
19The electrochemical discharge capacity that metal hydride-nickel cell had that the type cathode hydrogen storage material prepares is higher than commercial metals hydride-nickel-based battery far away.
As Pr of the present invention
5Co
19The example of type cathode hydrogen storage material, atomic ratio one-tenth is grouped into and can be:
La
0.64Nd
0.1Dy
0.01Mg
0.25Ni
3.27Al
0.13；
La
0.63Nd
0.1Dy
0.02Mg
0.25Ni
3.27Al
0.13；
La
0.62Nd
0.1Dy
0.03Mg
0.25Ni
3.27Al
0.13；
La
0.61Nd
0.1Dy
0.04Mg
0.25Ni
3.27Al
0.13；
La
0.60Nd
0.1Dy
0.05Mg
0.25Ni
3.27Al
0.13；
La
0.54Nd
0.2Dy
0.01Mg
0.25Ni
3.27Al
0.13；
La
0.53Nd
0.2Dy
0.02Mg
0.25Ni
3.27Al
0.13；
La
0.52Nd
0.2Dy
0.03Mg
0.25Ni
3.27Al
0.13；
La
0.51Nd
0.2Dy
0.04Mg
0.25Ni
3.27Al
0.13；
La
0.50Nd
0.2Dy
0.05Mg
0.25Ni
3.27Al
0.13；
La
0.44Nd
0.3Dy
0.01Mg
0.25Ni
3.27Al
0.13；
La
0.43Nd
0.3Dy
0.02Mg
0.25Ni
3.27Al
0.13；
La
0.42Nd
0.3Dy
0.03Mg
0.25Ni
3.27Al
0.13；
La
0.41Nd
0.3Dy
0.04Mg
0.25Ni
3.27Al
0.13Or
La
0.40Nd
0.3Dy
0.05Mg
0.25Ni
3.27Al
0.13Or the like.
Preferably, Pr of the present invention
5Co
19The type cathode hydrogen storage material is La
0.75-x-yNd
xDy
yMg
0.25Ni
3.27Al
0.13, 0.1≤x≤0.2,0.01≤y≤0.03 wherein.
Wherein, most preferred Pr
5Co
19The type cathode hydrogen storage material is La
0.53Nd
0.2Dy
0.02Mg
0.25Ni
3.27Al
0.13
Pr of the present invention
5Co
19The type cathode hydrogen storage material can adopt conventional smelting method for preparing.
For example; it can be La: Nd: Dy: Mg: Ni: Al=0.75-x-y: x: y with mol ratio: 0.25: 3.27: 0.13 (0.1≤x≤0.3; carry out melting and be cast into ingot casting 0.01 raw material≤y≤0.05) is inserted the vaccum sensitive stove that vacuumizes the back and feed argon shield; then; ingot casting is carried out homogenizing in the heat-treatment furnace that vacuumizes afterwards and feed argon shield handle; treatment temperature is 1020 ℃, and temperature retention time is 8 hours, treats to take out ingot casting again behind the stove cool to room temperature.
Pr of the present invention
5Co
19The type cathode hydrogen storage material can be used for preparing the negative pole of Ni-MH battery.Adopt Pr of the present invention
5Co
19The type cathode hydrogen storage material has very high charge discharge capacity as the Ni-MH battery of negative pole.
With the AB that sells in the market
5The type hydrogen storage material is (as the traditional cathode hydrogen storage material MmNi for preparing with identical smelting technology
3.55Co
0.75Mn
0.4Al
0.3) compare Pr of the present invention
5Co
19Type cathode hydrogen storage material La
0.75-x-yNd
xDy
yMg
0.25Ni
3.27Al
0.13The charge/discharge capacity of (0.1≤x≤0.3,0.01≤y≤0.05) significantly improves, and good cycle life is arranged.Correspondingly, adopt Pr of the present invention
5Co
19The charge discharge capacity that Ni-MH battery had that the type cathode hydrogen storage material prepares is higher than commercially available Ni-MH battery far away.
Embodiment
Below in conjunction with embodiment the present invention is launched further description.But should be appreciated that following execution mode only is used for the present invention is illustrated and is not in order to limit scope of the present invention.
Percentage by weight according to each element of alloy in the table 1 is prepared burden; the alloy raw material for preparing is carried out the melting casting in the induction furnace that vacuumizes afterwards and feed argon shield; then ingot casting being carried out homogenizing in the heat-treatment furnace that vacuumizes back feeding argon shield handles; treatment temperature is 1020 ℃; temperature retention time is 8 hours, treats to take out ingot casting behind the stove cool to room temperature.
The composition of table 1 embodiment of the invention and prior art is (wt%) relatively
The method of testing of electrochemistry capacitance is as follows: the hydrogen bearing alloy steel ingot after at first homogenizing being handled becomes less than 200 purpose alloyed powders in grinding at room temperature, then will be less than 200 purpose negative alloy powder 0.25g and nickel powder mixed by 1: 4, and add an amount of poly-vinyl alcohol solution as binding agent, be cold-pressed into diameter and use [the Ni (OH) that used positive electricity is very identical with Ni-MH battery as negative electrode for the cake of (d=15mm)
2-NiOOH] electrode, the Capacity design of positive electrode is the capacity far above negative electrode, so that negative electrode material reaches fully saturated when charging, [Hg/HgO/6M KOH] is reference electrode.In the electrode performance test process, at first storage hydrogen negative material is fully activated 30 ℃ of current densities with 60mA/g, the activation system is as follows: the current density charging 450min that adopts 60mA/g, paused 15 minutes in the charging back, then with the current density of 60mA/g discharge into the negative electrode current potential with respect to the electrode potential of reference electrode for till-0.5 volt, carry out the next round charge and discharge cycle again.Increase along with the activation number of times, capacity of negative plates will progressively increase and be relatively stable following after reaching a maximum, this moment, activation finished, and this maximum is decided to be the hydrogen storage capability of material under 30 ℃, will obtain the needed charge and discharge cycles number of times of this maximum and be called the activation number of times.
The Pr of each execution mode of the present invention that said method is recorded
5Co
19The maximum electrochemistry capacitance test result of type hydrogen storage material under 30 ℃, 60mA/g charging and discharging currents density and traditional AB of activation number of times and prior art
5Electrochemistry capacitance and the activation number of times of type hydrogen storage material under 30 ℃, 60mA/g charging and discharging currents density listed in the table 2.
Test for cycle life, charging and discharging currents density is chosen as 300mA/g, method of testing is as follows: at first adopt the current density of 60mA/g to activate by the method for above-mentioned test capacity with the activation number of times at 30 ℃ specimen, after activation is good, 30 ℃ of current densities that adopt 300mA/g to the storage hydrogen negative material 85min that charges, paused 15 minutes in the charging back, then with the current density of 300mA/g discharge into the negative electrode current potential with respect to the electrode potential of reference electrode for till-0.5 volt, carrying out next round again fills, discharge cycles, in order to contrast conveniently, the cycle life of sample is defined as cycle-index when its capacity under this experiment condition drops to 160mAh/g, and its test result all is given in the table 2.
Activity function and electrochemistry capacitance (mAh/g) and under 30 ℃, 300mA/g charging and discharging currents density the cycle life relatively (by capacity is 160mAh/g) of table 2 hydrogen bearing alloy under 30 ℃, 60mA/g charging and discharging currents density
By the data of table 2 as can be known: substitute La with Nd and Dy,, can improve the electrochemistry capacitance and the cycle life of alloy, but along with the increase that substitutes amount, the electrochemistry capacitance and the cycle life of alloy reduce on the contrary when substituting amount more after a little while, but with conventional AB
5Type alloy phase ratio, though the life-span is poor slightly, capacity has very big increase, its high electrochemistry capacitance has reached 375mAh/g, far above the AB that sells in the market
5The electrochemistry capacitance value of type hydrogen storage material.
In sum, be in the hydrogen storage material at La-Mg-Ni, suitable selection atom proportioning, and with Nd and the alternative La of Dy, when substituting amount more after a little while, the Pr that is suitable for the Ni-MH battery use that available can be excellent
5Co
19Type high power capacity, the long-life cathode hydrogen storage material that uses for nickel-hydrogen battery.Its electrochemistry charge and discharge capacity reaches as high as 375mAh/g, far above present commercially available AB
5The electrochemistry charge and discharge capacity of type hydrogen storage alloy.
Claims (6)
1.Pr
5Co
19The type cathode hydrogen storage material, its atomic ratio one-tenth is grouped into and is expressed from the next:
La
0.75-x-yNd
xDy
yMg
0.25Ni
3.27Al
0.13, wherein 0.1≤x≤0.3,0.01≤y≤0.05.
2. Pr according to claim 1
5Co
19The type cathode hydrogen storage material is characterized in that, 0.1≤x in the following formula≤0.2,0.01≤y≤0.03.
3. Pr according to claim 1
5Co
19The type cathode hydrogen storage material is characterized in that, described Pr
5Co
19The type cathode hydrogen storage material is shown below:
La
0.64Nd
0.1Dy
0.01Mg
0.25Ni
3.27Al
0.13；
La
0.63Nd
0.1Dy
0.02Mg
0.25Ni
3.27Al
0.13；
La
0.62Nd
0.1Dy
0.03Mg
0.25Ni
3.27Al
0.13；
La
0.61Nd
0.1Dy
0.04Mg
0.25Ni
3.27Al
0.13；
La
0.60Nd
0.1Dy
0.05Mg
0.25Ni
3.27Al
0.13；
La
0.54Nd
0.2Dy
0.01Mg
0.25Ni
3.27Al
0.13；
La
0.53Nd
0.2Dy
0.02Mg
0.25Ni
3.27Al
0.13；
La
0.52Nd
0.2Dy
0.03Mg
0.25Ni
3.27Al
0.13；
La
0.51Nd
0.2Dy
0.04Mg
0.25Ni
3.27Al
0.13；
La
0.50Nd
0.2Dy
0.05Mg
0.25Ni
3.27Al
0.13；
La
0.44Nd
0.3Dy
0.01Mg
0.25Ni
3.27Al
0.13；
La
0.43Nd
0.3Dy
0.02Mg
0.25Ni
3.27Al
0.13；
La
0.42Nd
0.3Dy
0.03Mg
0.25Ni
3.27Al
0.13；
La
0.41Nd
0.3Dy
0.04Mg
0.25Ni
3.27Al
0.13Or
La
0.40Nd
0.3Dy
0.05Mg
0.25Ni
3.27Al
0.13。
4. Pr according to claim 3
5Co
19The type cathode hydrogen storage material is characterized in that, described Pr
5Co
19The type cathode hydrogen storage material is shown below: La
0.53Nd
0.2Dy
0.02Mg
0.25Ni
3.27Al
0.13
5. any described Pr in the claim 1～4
5Co
19The application of type cathode hydrogen storage material in the preparation nickel-hydrogen battery negative pole.
6. application according to claim 5 is characterized in that described Ni-MH battery is a high-capacity nickel-hydrogen battery.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN200810181720A CN101752557A (en) | 2008-12-04 | 2008-12-04 | Pr5Co19 type cathode hydrogen storage material and application thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN200810181720A CN101752557A (en) | 2008-12-04 | 2008-12-04 | Pr5Co19 type cathode hydrogen storage material and application thereof |
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| Publication Number | Publication Date |
|---|---|
| CN101752557A true CN101752557A (en) | 2010-06-23 |
Family
ID=42479181
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN200810181720A Pending CN101752557A (en) | 2008-12-04 | 2008-12-04 | Pr5Co19 type cathode hydrogen storage material and application thereof |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102723450A (en) * | 2012-05-25 | 2012-10-10 | 南京航空航天大学 | Automatic temperature control battery box of electric automobile |
| CN103094531A (en) * | 2011-11-01 | 2013-05-08 | 北京宏福源科技有限公司 | La-Mg-Ni negative electrode hydrogen storage material used in power-type nickel-metal hydride battery |
| CN107845779A (en) * | 2017-10-31 | 2018-03-27 | 包头中科轩达新能源科技有限公司 | A kind of Pr5Co19 types superlattices Nd-Mg-Ni systems single phase alloy electrode material and preparation method thereof |
-
2008
- 2008-12-04 CN CN200810181720A patent/CN101752557A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103094531A (en) * | 2011-11-01 | 2013-05-08 | 北京宏福源科技有限公司 | La-Mg-Ni negative electrode hydrogen storage material used in power-type nickel-metal hydride battery |
| CN103094531B (en) * | 2011-11-01 | 2015-11-11 | 北京宏福源科技有限公司 | A kind of power-type La-Mg-Ni negative hydrogen storage material for nickel-hydrogen batteries |
| CN102723450A (en) * | 2012-05-25 | 2012-10-10 | 南京航空航天大学 | Automatic temperature control battery box of electric automobile |
| CN102723450B (en) * | 2012-05-25 | 2015-08-12 | 南京航空航天大学 | The automatic temperature-controlled battery case of electric automobile |
| CN107845779A (en) * | 2017-10-31 | 2018-03-27 | 包头中科轩达新能源科技有限公司 | A kind of Pr5Co19 types superlattices Nd-Mg-Ni systems single phase alloy electrode material and preparation method thereof |
| CN107845779B (en) * | 2017-10-31 | 2020-02-21 | 包头中科轩达新能源科技有限公司 | Pr5Co19 type superlattice Nd-Mg-Ni series single-phase alloy electrode material and preparation method thereof |
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